Conformable holographic labels

ABSTRACT

This invention relates to a facestock comprising a polymeric film, and a holographic layer on a surface of the facestock, wherein the film is conformable. The invention also relates to label stocks prepared from the facestocks, and labels made therefrom. The labels are useful on squeezable containers. An advantage of these labels is that there is little or no cracking or flaking of the holographic image.

FIELD OF THE INVENTION

[0001] This invention relates to labels and facestocks that areconformable and contain a holographic image. More specifically, thisinvention relates to a label and facestock that contain a holographicimage layer which is conformable and/or squeezable, e.g. the holographicimage does not crack or flake.

BACKGROUND OF THE INVENTION

[0002] Holograms and other types of defraction gratings are commonlyattached to documents or other articles. Holograms have been used assecurity means in documents as well as credit cards to authenticatetheir genuineness and increase the difficulty of counterfeiting thosearticles. Holograms have also been attached to printed documents andother articles for decorative and aesthetic reasons, as well. Forconsumer goods, hologram containing labels provide an eye-catchingdisplay for products.

[0003] One problem associated with the use of holograms in labels hasbeen that holograms tend to be stiff. The hologram within the labeltends to crack or flake. In labels, holograms may provide market appealbut have traditionally been avoided due to the problem with the imagebeing destroyed during processing or during the use of the productcontaining the holographic label. It is desirable to have a hologramwithin a label where the image is conformable to a squeezable bottle orsqueezable container.

SUMMARY OF THE INVENTION

[0004] This invention relates to a facestock comprising a polymericfilm, and a holographic layer on a surface of the facestock, wherein thefilm is conformable. The invention also relates to label stocks preparedfrom the facestocks, and labels made therefrom. The labels are useful onsqueezable containers. An advantage of these labels is that there islittle or no cracking or flaking of the holographic image.

BRIEF DESCRIPTION OF THE DRAWINGS

[0005]FIG. 1a is a cross-section of a facestock of the present inventioncomprising a film layer embossed with an image.

[0006]FIG. 1b is a cross section of a facestock of the present inventioncomprising a film layer and a holographic layer, having a reflectivematerial coating the whole surface of the holographic layer.

[0007]FIG. 1c is a cross section of a facestock of the present inventioncomprising a film layer and a holographic layer, having a reflectivematerial coating only the image area of the holographic layer.

[0008]FIG. 2 is a cross-section of a facestock of the present inventioncomprising a multilayer film having two layers and a holographic layer.

[0009]FIG. 3 is a cross-section of a facestock of the present inventioncomprising a multilayer film having three layers and a holographiclayer.

[0010]FIG. 4 is a cross-section of a labelstock in accordance with thepresent invention comprising the facestock illustrated in FIG. 1b withan adhesive layer and a release liner.

[0011]FIG. 5 is a cross-section of a labelstock in accordance with thepresent invention comprising the facestock illustrated in FIG. 3 with anadhesive layer and a release liner.

[0012]FIG. 6 is a cross-section of a labelstock in accordance with thepresent invention in which a protective layer overlies the holographiclayer.

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0013] As described herein, the present invention relates to labels andfacestocks for use therein. The labels are useful on deformable andsqueezable bottles. The deformation may be permanent as in toothpastetubes or non-permanent, as in hair shampoo bottles, toothpaste tubes,hand lotion bottles and tubes, etc.

[0014] As used herein, the term “conformable” means the film or labelhas the ability to yield to the contours of a curved or rough surface. Aconformable holographic label will conform to the container or substrateto which it is applied without cracking or flaking of the holographicimage.

[0015] Holographic Layer

[0016] The facestock and label stock contain a holographic layer. Asshown in FIG. 1a, facestock 10 has a polymeric film layer 11, having anupper surface and a lower surface, wherein the lower surface is adheredto a holographic layer 12. The bottom surface of polymeric film 11 maybe adhered directly to the holographic layer 12, or adhered indirectlyto the holographic layer through either a tie layer or adhesive layer(not shown). The holographic layer 12 has an image 13 on the surfaceopposite of the polymeric film layer 11.

[0017] In one embodiment, the holographic layer having an upper surfaceand an image surface, has a reflective material on the image surface. Asshown in FIG. 1b, the polymeric film 11 is adhered to the holographiclayer 12, having upper surface 15 and image surface 16 having image 13.A reflective material 14, such as aluminum or other material known tothose in the art covers the image surface 16 and forms the hologram onthe surface of holographic layer 12.

[0018] In another embodiment, as shown in FIG. 1c, the facestock haspolymeric layer 11 adhered to holographic layer 12, having image 13. Thereflective material 14 covers only a portion of the image surface 16 ofholographic layer 12, namely the area of the image 13.

[0019] The holographic layer contains an image that is treated with areflective materials as is known to those in the art. The image may beformed on the polymeric facestock by embossing the film and thenmetalizing the image area or the entire image surface of the film. Theimage may also be formed using a liquid casting resin. This resin can bea radiation curable resin that is coated onto the facestock film. Theimage is imparted to the casting resin using a hologram master or othermeans known to those in the art. The radiation curable resins includeCellofilms, such as Cellofilm C-200 and Radcure resins, such as Radcure#801.

[0020] The radiation curable resins are generally used as an oligomer.The oligomers are available commercially from a variety of sources.Urethane acrylate oligomers are available from Morton Thiokol under thedesignations Uvithane 782 and Uvithane 783, and from Polymer SystemsCorp., Orlando, Fla. under the designation PURELAST. Ebecryl 270 is anacrylated aliphatic urethane oligomer available from UCB Radcure,Atlanta, Ga. Epoxy acrylate oligomers are available, for example, fromUCB Radcure, Atlanta, Ga. under the designations Novacure 3600 and fromShell Chemical Company under the designation Epocryl 25A60. AlthoughEpocryl 25A60 contains some volatile solvent, the product can be mixedwith an acrylate monomer such as, for example, 1,6-hexanedioldiacrylate, and the solvent originally present can be removed. Anexample of a commercially available acrylic acrylate oligomer isNovacure 6700 from UCB Radcure. An example of a commercially availablepolyamine acrylate oligomer is Novacure 7100 from UCB Radcure. Thisacrylate functional oligomeric amine is a liquid having a viscosity inthe range of 500 to 1500 CPS at 25° C. and a theoretical molecularweight of 800, and the oligomer contains less than 10% of hexanedioldiacrylate.

[0021] The process of imparting the image to the holographic layer andmaterials used therein, including materials used as the casting resin,are described in U.S. Pat. Nos. 4,728,377 (Gallagher); 4,913,858 (Malliket al); 4,933,120 (D'Amato); 5,003,915 (D'Amato); 5,083,850 (Miekk etal), 5,116,548 (Mallik); 4,906,315 (McGrew); 5,948,199 (McGrew);5,164,227 (Miekka et al); and 5,643,678 (Boswell), the entiredisclosures of which are hereby incorporated by reference herein.

[0022] In another embodiment, the hologram image is prepared using afoil/composite sheet. U.S. Pat. Nos. 5,810,957, 5,783,017, 5,759,683,5,753,349, 5,674,580, 5,670,003, 5,643,678 and 5,464,690 relate tofoil/composite sheets having a holographic image or diffraction gratingimage impressed into the foil and one or more of the composite layers.These patents disclose, e.g., hot stamping a chip containing theholographic image directly on a substrate such as a document. Thefoil/composite sheet disclosed in 5,810,957, for example, includes inorder, a plastic carrier film, a release coating, a hard lacquercoating, a soft lacquer coating, a layer of metal and an embossmentreceiving coating. The soft lacquer coating, the metal layer and theembossment receiving coating are embossed with the holographic imagewhen a heated embossing shim applied under pressure against theembossment receiving layer. A heat activatable adhesive is thereafterapplied to the embossment receiving coating, to apply the chip to thedocument. The embossment receiving coating, which may also be referredto as a release coating, may be a wax such as a microcrystalline wax orpartially saponified montan wax or may be a siloxane. The metal is,e.g., aluminum. The soft lacquer coating may be a thermosofteningpolymer which contains an acrylic or nitrocellulose or a chlorinatedrubber. The other patents in this group disclose similar foil/compositesheet constructs in which a holographic image is applied to thefoil/composite sheet to form a chip, and thereafter the chip is appliedto a document or other substrate by, e.g., hot stamping. Each of U.S.Pat. Nos. 5,810,957; 5,783,017; 5,759,683; 5,753,349; 5,674,580;5,670,003; 5,643,678 and 5,464,690 is incorporated herein by referencefor the teachings relating to forming such hot-stampable holographicimages on foil/composite sheets.

[0023] Polymeric Facestocks

[0024] The facestocks comprise a holographic layer and a polymeric film.The film may be a monolayer polymeric film or a multilayer polymericfilm. Such multilayer films generally contain a base layer andoptionally, one or more additional layers. The layers may be laminatedtogether by coextrusion or may be adhered together using adhesives. Inone embodiment, the facestocks of the present invention have improvedmachine direction Gurley stiffness and die-cuttability, particularlywhen the polymeric film has been oriented in the machine direction only.When the polymeric film is a multilayer film, the base layer only may beoriented or all layers of the multilayer film may be oriented in themachine direction. A multilayer film of the present invention in whichonly the base layer has been machine direction oriented can be obtainedby preparing a machine direction oriented polypropylene film andthereafter coextrusion coating a tie layer and the first skin layer overthe oriented polypropylene layer to form a three layer film. More often,however, the entire film is machine direction oriented after formation,preferably by coextrusion.

[0025] In one embodiment, the base layer of a multilayer film and/or theentire multilayer film is oriented in the machine direction at a stretchratio of at least about 2:1, and/or at a stretch ratio of from about 3:1to about 9:1. In another embodiment, the single or multilayer film isoriented in a machine direction at a ratio of about 4:1 to about 6:1.The oriented films are then usually heat set or annealed to providedimensional stability (i.e., to prevent shrinking, relaxing or anydistortion of the film).

[0026] The thickness of the facestock will range from about 0.5 mils(12.5 microns) to about 10 mils (250 microns) depending upon theanticipated utility of the facestock. More often, however, thefacestocks of the present invention will have a thickness of less than 6mils (150 microns). Facestock thicknesses of from about 1 to about 6mils (25 to 150 microns), more often from about 1 to about 4 mils (25 to100 microns) and most often from about 1.5 to about 2.5 mils (37.5 to62.5 microns) are particularly useful for preparing labels to be appliedto rigid and flexible substrates. As noted earlier, a particular featureof the facestocks of the invention is that very thin films (i.e., 1 to2.5 mils, or 25 to 62.5 microns) can be prepared and are useful informing labels. Here and elsewhere in the specification and claims therange and ratio limits may be combined.

[0027] The film may be formed from any polymer or combination ofpolymers that are useful in forming polymeric facestocks and labels. Thepolymeric film may be derived from polymers that include polystyrenes,polyolefins, polyamides, polyesters, polycarbonates, polyvinyl alcohol,poly(ethylene vinyl alcohol), polyurethanes, polyacrylates, poly(vinylacetates), ionomers and mixtures thereof. In one embodiment, thepolymeric film material is a polyolefin. In another embodiment, thepolyolefin film materials generally are characterized as having a meltindex or melt flow rate of less than 30, more often less than 20, andmost often less than 10 as determined by ASTM Test Method 1238. Thepolymeric films of the invention are conformable.

[0028] In one embodiment, the polymeric film is (a) a propylenehomopolymer or copolymer, (b) polyethylene or (c) a blend of (i) apropylene homopolymer or polyethylene and (ii) at least one propylenecopolymer. When blends of homopolymers and copolymers are used, theblends may comprise from about 5% to about 95% of the homopolymer andcorrespondingly from about 95% to about 5% by weight of the copolymer.The propylene homopolymers that may be utilized as the base materialeither alone or in combination with a propylene copolymer as describedherein, include a variety of propylene homopolymers such as those havingmelt flow rates (MFR) from about 1 to about 20 as determined by ASTMTest D1238, condition L. Propylene homopolymers having an MFR of atleast about 4, or at least about 8, are particularly useful and providefacestocks having improved die-cuttability. Useful propylenehomopolymers also may be characterized as having densities in the rangeof about 0.88 to about 0.92 g/cm³.

[0029] A number of useful propylene homopolymers are availablecommercially from a variety of sources. Some of the useful homopolymersare listed and described in the following Table I. TABLE I CommercialPropylene Homopolymers Commercial Melt Flow Designation Company g/10 minDensity (g/cm³) WRD5-1057 Union Carbide 12.0 0.90 DX5E66 Union Carbide8.8 0.90 5A97 Union Carbide 3.9 0.90 Z9470 Fina 5.0 0.89 Z9470HB Fina5.0 0.89 Z9550 Fina 10.0 0.89 6671XBB Fina 11.0 0.89 3576X Fina 9.0 0.893272 Fina 1.8 0.89 SF6100 Montell 11.0 0.90

[0030] The propylene copolymers that may be utilized in the base layergenerally comprise copolymers of propylene and up to about 40% by weightof at least one alpha-olefin selected from ethylene and alpha-olefinscontaining from 4 to about 8 carbon atoms. Examples of usefulalpha-olefins include ethylene, 1-butene, 1-pentene, 4-methyl-1-pentene,1-hexene, 1-heptene, and 1-octene. More often, the copolymers ofpropylene that are utilized in the present invention comprise copolymersof propylene with ethylene, 1-butene or 1-octene. The propylenealpha-olefin copolymers useful in the present invention include randomas well as block copolymers, although the random copolymers generallyare preferred. Blends of the copolymers as well as blends of thecopolymers with propylene homopolymers can be utilized as thecomposition for the base layer. In one preferred embodiment, thepropylene copolymers are propylene-ethylene copolymers with ethyleniccontents of from about 0.2% to about 10% by weight. In one embodiment,the ethylene content is from about 3% to about 10% by weight and morepreferably from about 3% to about 6% by weight. With regard to thepropylene-1-butene copolymers, 1-butene contents of up to about 15% byweight are useful. In one embodiment, the 1-butene content generally mayrange from about 3% by weight up to about 15% by weight, and in otherembodiments, the range may be from about 5% to about 15% by weight.Propylene-1-octene copolymers useful in the present invention maycontain up to about 40% by weight of 1-octene. More often, thepropylene-1-octene copolymers will contain up to about 20% by weight of1-octene.

[0031] In one embodiment, the propylene copolymers used in the presentinvention are obtained by copolymerization of propylene with analpha-olefin such as ethylene or 1-butene using single-site metallocenecatalysts. A list of some useful commercially available propylenecopolymers is found in the following Table II. The propylene copolymersuseful in the invention have an MFR of from about 1 to about 20,preferably from about 1 to about 12. Improved die-cuttability isobtained when the propylene copolymer has an MFR of at least about 4.

[0032] In one embodiment, the polymeric film is characterized as beingclear or crystal clear. The film is a machine direction only orientedfilm having an opacity of about 10% and a haze of about 10% or less inthe machine direction and cross direction. In one embodiment, the hazeis about 5% or less. The opacity of the film is measured using TAPPITest 425, and the haze is measured in accordance with ASTM Test MethodD-1003. The percent of ethylene in the propylene-ethylene copolymers andthe percent of 1-butene in the propylene-1-butene copolymers, and thedraw or stretch ratio in the machine-direction are controlled and may bevaried to provide the desired clarity.

[0033] In general, as the concentration of ethylene or 1-butene in thepropylene copolymers increases, the haze of the film decreases. Forexample, when the copolymer film comprises a polypropylene-ethylenecopolymer that contains from about 5% to about 6% of ethylene, clearfilms can be obtained at stretch rations in the machine direction ofabout 7 or less, and more often of about 5 or less. A stretch ratio ofabout 4 or less is useful when the copolymer is a propylene-ethylenecopolymer that contains from about 3% to about 6% of ethylene. Inparticular, a propylene-ethylene copolymer containing about 5,5%ethylene provides a clear film when oriented in the machine0direction ata stretch ration of about 5:1. When the copolymer film is apropylene-ethylene copolymer containing 3.2% ethylene, a stretch rationof about 4:1 provides a clear film. Clear films also are obtained when apropylene-1-butene copolymer containing about 8% to 14% 1-butene aredrawn at a stretch ratio of about 4:1 and 5:1.

[0034] In one embodiment, the polymeric film comprises a monolayer of ablend of (a) a propylene homopolymer or copolymer and (b) analkylene-alkyl-acrylate or methacrylate copolymer. The alkylene can bean a-olefin containing from about 2 to about 8 carbon atoms. Thealkyl-acrylate can be a C₁-C₈ alkyl acrylate or methacrylate. In oneembodiment, the alkylene-alkyl-acrylate is ethylene butyl acrylatecopolymer. The amount of propylene homopolymer or copolymer in the blendis generally within the range of 40-90% by weight and the amount ofalkylene-alkyl-acrylate or methacrylate copolymer in the blend isgenerally within the range of 10-60% by weight. TABLE II CommercialPropylene Copolymers Commercial % % Melt Flow Rate Density Name SourceEthylene 1-Butene (g/10 mins) (g/cm³) DS4D05 Union — 14 6.5 0.890Carbide DS6D20 Union 3.2 — 1.9 0.890 Carbide DS6D81 Union 5.5 — 5.0 NACarbide SRD4-127 Union —  8 8.0 NA Carbide SRD4-104 Union — 11 5.0 NACarbide SRD4-105 Union — 14 5.0 NA Carbide

[0035] In another embodiment of the invention, the film may comprise apolyethylene, such as low density, linear low density, high density,very high density polyethylene as well as ethylene copolymers. In oneembodiment, the polyethyene may be oriented in the machine direction.Stretch ratios may range from about 2:1 to about 9:1.

[0036] The film may contain other additives to modify the properties ofthe base layer and the facestock film. For example, colorants may beincluded in the base layer such as TiO₂, CaCO₃, etc. The presence ofsmall amounts of TiO₂, for example, results in a white facestock.Antiblock agents also can be included in the base layer. AB-5 is anantiblock concentrate available from A. Schulman Inc., 3550 West MarketStreet, Akron, Ohio 44333, that comprises 5% solid synthetic amorphoussilica in 95% low density polyethylene. ABPP05SC is an antiblockconcentrate from Schulman containing 5% of the synthetic amorphoussilica in a propylene copolymer. The amount of antiblock agent (silica)present in the base layer may range from about 500 to about 5000 ppm,with amounts of about 1000 ppm being preferred. In some embodiments, italso is advantageous to add flexible polyolefins to the base layer toreduce graininess and reduce cross-direction (CD) splitting. Usefulflexible polyolefins (polypropylene copolymers) are available fromRexene under the trade designation W-105, W-107, and W-113.

[0037] As illustrated in FIG. 2, the film may be a multilayer film.Facestock 20 comprises a base layer 21 having an upper and lowersurface. The upper surface of base layer 21 is adhered to a skin layer24. The base layer 21 may be adhered to the skin layer directly, as istypical for coextruded films, or indirectly, through a tie layer oradhesive layer. The lower surface of the base layer is adhered to theholographic layer 22 having image 23 therein.

[0038] The multilayer films of the present invention may furthercomprise at least one tie layer positioned between the base layer andthe first skin layer. The tie layer may comprise any polymeric materialthat improves the adhesion of the first skin layer to the base layer. Inone embodiment, the tie layer comprises a mixture of a propylenehomopolymer or copolymer and a soft polar additive (“SPA”) such asethylene vinyl acetate copolymer (EVA). Any of the propylenehomopolymers or copolymers described above as useful in the base layercan be used in the tie layer. The weight ratio of the propylene polymeror copolymer and the SPA in the blend may range from about 50/50 to60/40. The soft polar additives generally comprise random copolymers ofan olefin and a more polar moiety. In addition to the preferred softpolar additive, which is ethylene vinyl acetate copolymer (EVA), the tielayers may include other soft polar additives such as ethylenemethylacrylate (EMA) and acrylonitrile butadiene rubber.

[0039] Particular examples of such blends useful as the tie layerinclude a blend containing 50% EVA and 50% of a random propylenecopolymer containing about 6% ethylene; a blend of 60% EVA and 40% of apropylene homopolymer; and 50% EMA and 50% of a propylene homopolymer.Specific examples of ethylene vinyl acetate copolymers useful in thepresent invention are those containing 18% vinyl acetate and 28% vinylacetate.

[0040] The tie layers also may comprise polar additives such as ethylenemethylacrylate (EMA) without any additional propylene polymer. Examplesof a useful commercially available EMA include EM-803-115 (meltindex=3.5), EM 806-009 (melt index=6.0) and EM 802-009 (melt index=2.0)available from Equistar, 1221 McKinney, Houston, TX 77252.

[0041] Examples of thermoplastic film forming polymers that can beutilized in the skin layer, either alone or in combination with otherthermoplastic polymers include polyolefins (linear or branched),polyamides, polystyrenes, nylon, polyesters, polyester copolymers,polyurethanes, polysulfones, polyvinylidine chloride, styrene-maleicanhydride copolymers, styrene-acrylonitrile copolymers, ionomers basedon sodium or zinc salts of ethylene methacrylic acid, polymethylmethacrylates, cellulosics, fluoroplastics, acrylic polymers andcopolymers, polycarbonates, polyacrylonitriles, and ethylene-vinylacetate copolymers. Some specific examples of thermoplastics useful asthe second skin layer include acrylates such as ethylene methacrylicacid, ethylene methyl acrylate, ethylene acrylic acid and ethylene ethylacrylate. In one embodiment, the skin layer comprises a mixture of apolyethylene and a propylene homopolymer or copolymer. The selection ofa particular polymer for the skin layer is dependent on the propertiesand characteristics that are to be added by the presence of the skinlayer. The polymer for the skin layer should be compatible with thepolymer of the base layer to provide sufficient adhesion to the baselayer in the absence of a tie layer.

[0042] In FIG. 2, the lower surface of base layer 21 is also adhered toholographic layer 22, having holographic image 23. As described above,the adherence may be direct or indirect through the use of the tielayer. For convenience, the reflective layer is not shown in FIG. 2. Aspreviously described, the reflective material may cover only a portionor all of the holographic layer.

[0043] In one embodiment, the skin layer that is bonded to the uppersurface of the base layer by a tie layer in the multilayer filmfacestocks of the present invention comprises at least one polyethylenehaving a density of about 0.940 g/cm³ or less. Such polyethylenesgenerally are referred to in the art as low density or medium densitypolyethylenes, and these polyethylene homopolymers can be prepared bytechniques well known to those skilled in the art including highpressure, free radical catalyzed processes and processes usingmetallocene catalysts. Low density polyethylenes and metallocenecatalyzed processes for preparing such polyethylenes are described inU.S. Pat. Nos. 5,358,792; 5,462,809; 5,468,440; 5,475,075; and5,530,054. Each of these patents is hereby incorporated by reference forits disclosure of metallocene catalysts, polyethylenes, and methods forpreparing polyethylenes. Metallocene-catalyzed polyethylene generallyhave a density of from about 0.850 to about 0.925 g/cm³, and more oftenfrom about 0.870 to about 0.920 g/cm³.

[0044] Useful ethylene homopolymers for the skin layer include thosehaving densities of from 0.850 up to about 0.940 or less. Polyethyleneshaving densities of from 0.850 to about 0.925 g/cm³ generally arereferred to as low density polyethylenes, and polyethylenes havingdensities between about 0.925 and 0.940 are referred to in the art asbeing medium density polyethylenes. The low and medium densitypolyethylenes useful in the skin layer also may be characterized ashaving a melt index (as determined by ASTM Test D1238, condition E) inthe range of from 0.5 to about 25. In addition to the above densities,and melt indices, the low density polyethylenes may be characterized bytensile strengths of between about 2200 to about 3200 psi (typicallyabout 2700 psi), and the medium density polyethylenes may becharacterized as having tensile strengths of between about 3000 andabout 4000 psi (typically about 3400 psi). The determination of whethera low density or medium density polyethylene is to be utilized as theskin layer is based in part on the film thickness of the skin and theoverall thickness of the facestock. Thicker films of lower densitypolyethylenes generally are preferred because of the softness andrelatively low tensile strength of the low density polyethylenes.Conversely, thinner films of medium density polyethylenes can beutilized in the facestocks of the present invention.

[0045] Low and medium density polyethylene useful in the skin layer ofthe facestock of this invention are available commercially from avariety of sources. Examples of useful polyethylenes are summarized inthe following Table III. TABLE III Commercial Polyethylenes CommercialMelt Index Designation Company (g/10 mins) Density (g/cm³) Rexene 1017Rexene 2.0 0.920 Rexene 1058 Rexene 5.5 0.922 Rexene 1080 Rexene 2.00.930 Rexene 2030 Rexene 5.0 0.919 Rexene 2034 Rexene 7.5 0.925 Rexene2038 Rexene 9.0 0.917 Rexene 2040 Rexene 12.0 0.917 Rexene 2049 Rexene20.0 0.917 NA-334 Equistar 6.0 0.918 NA-217 Equistar 5.5 0.923 NA285-003 Equistar 6.2 0.930 Exact 3027 Exxon 3.5 0.900 Exact 3022 Exxon9.0 0.905 Exact 3139 Exxon 7.5 0.900 SLP 9053 Exxon 7.5 0.900 AffinityPF1140 Dow Chemical 1.6 0.895

[0046] The skin layer may also contain other additives such as theantiblock agents described above for the base layer. The amount of theantiblock agent or agents in the first skin layer may range from about500 to about 5000 ppm with amounts of about 1000 ppm generally beingpreferred.

[0047] Various nucleating agents and pigments can be incorporated intothe film formulations of the present invention. Preferably thenucleating agents are incorporated into the base layer and/or the tielayer, but not in the first skin layer. The amount of nucleating agentadded should be an amount sufficient to provide the desired modificationof the crystal structure while not having an adverse effect on thedesired properties of the facestock. It is generally desired to utilizea nucleating agent to modify the crystal structure and provide a largenumber of considerably smaller crystals or spherulites to improve thetransparency (clarity), and stiffness, and the die-cuttability of thefilm. Obviously, the amount of nucleating agent added to the filmformulation should not have a deleterious affect on the clarity of thefilm. Nucleating agents that have been used heretofore for polymer filmsinclude mineral nucleating agents and organic nucleating agents.Examples of mineral nucleating agents include carbon black, silica,kaolin and talc. Among the organic nucleating agents that have beensuggested as useful in polyolefin films include salts of aliphaticmono-basic or di-basic acids or arylalkyl acids such as sodiumsuccinate, sodium glutarate, sodium caproate, sodium 4-methylvalerate,aluminum phenyl acetate, and sodium cinnamate. Alkali metal and aluminumsalts of aromatic and alicyclic carboxylic acids such as aluminumbenzoate, sodium or potassium benzoate, sodium beta-naphtholate, lithiumbenzoate and aluminum tertiary-butyl benzoate also are useful organicnucleating agents. Substituted sorbitol derivatives such as bis(benzylidene) and bis (alkylbenzilidine) sorbitols wherein the alkylgroups contain from about 2 to about 18 carbon atoms are usefulnucleating agents. More particularly, sorbitol derivatives such as1,3,2,4-dibenzylidene sorbitol, 1,3,2,4-di-para-methylbenzylidenesorbitol, and 1,3,2,4-di-para-methylbenzylidene sorbitol are effectivenucleating agents for polypropylenes. Useful nucleating agents arecommercially available from a number of sources. Millad 8C-41-10, Millad3988 and Millad 3905 are sorbitol nucleating agents available fromMilliken Chemical Co.

[0048] The amounts of nucleating agent incorporated into the filmformulations of the present invention are generally quite small andrange from about 100 to about 2000 or 4000 ppm of the total facestock.Preferably the amount of nucleating agent should not exceed about 2000ppm, and in one embodiment, a concentration of about 300 to 500 ppmappears optimum.

[0049] In one embodiment, the facestock film comprises a base layerhaving a skin layers on each of its surfaces. As shown in FIG. 3,facestock 30 includes base layer 31 having an upper and lower surface.The upper surface of the base layer 31 is adhered to a first skin layer34 and the lower surface is adhered to a second skin layer 35.Holographic layer 32 having image 33 is adhered to the lower surface ofsecond skin layer 35. A reflective material (not shown) may be coatedonto a portion of or the entire lower surface of the holographic layer32 with image 33.

[0050] The composition of the second skin layer 35 may be the same asthe first skin layer 34 or different from the composition of the firstskin layer. In one embodiment, the second skin layer may consistsessentially of the same polymers or blends as present in the first skinlayer, or the second skin layer may comprise a different polymers orblends. A particularly useful multilayer film is the coextruded productof a polypropylene skin layer, a blend of polypropylene and ethylenevinyl acetate (18% vinyl acetate) (weight ratio of 75:25) and a baselayer or propylene butene copolymer (3.2% butene), titanium dioxide, andcalcium carbonate (weight ratio of 50:30:20).

[0051] The multilayer film of the invention comprises, in oneembodiment, a base layer having an upper surface and a lower surface,and at least a first skin layer bonded to the upper surface of the baselayer by a tie layer wherein the base layer comprises (a) a propylenehomopolymer or copolymer, (b) a polyethylene, or (c) a blend of apropylene homopolymer and at least one propylene copolymer. The firstskin layer comprises (a) a propylene homopolymer or copolymer, (b) apolyethylene, or (c) a blend of a propylene homopolymer and at least onepropylene copolymer

[0052] The layers of the multilayered film of the facestock can beformed by a variety of techniques known to those skilled in the artincluding blown or cast extrusion, or extrusion coating or by acombination of these techniques. U.S. Pat. No. 5,186,782 (Freedman), andU.S. Pat. Nos. 5,242,650 (Rackovan et al) and 5,435,963 (Rackovan et al)disclose useful procedures for preparing multilayer films, and thesepatents are hereby incorporated in their entirety by reference herein.The layers can be formed by simultaneous extrusion from a suitable knowntype of coextrusion die, and the three layers are adhered to each otherin a permanently combined state to provide a unitary coextrudate.Alternatively, the base layer can be formed by extrusion of the baselayer on a substrate followed by coextrusion coating of the tie layerand first skin layer onto the base layer thereby forming a three layerstructure wherein the layers are adhered to each other in a permanentlycombined state. In another alternative embodiment, the three layers maybe separately formed by extrusion and thereafter laminated together bythe application of heat and pressure.

[0053] Generally, the base layer is relatively thick compared to thefirst skin layer and the tie layer. In another, although generally notpreferred embodiment, the first skin layer may be relatively thickcompared to the base layer and the tie layer. Accordingly, thicknessratios for the three layered films may range from about 90:5:5 to 5:5:90(base:tie:first skin). However, generally preferred thickness ratios forthe three layered films (base: tie: first skin) include 90:5:5;80:10:10; 70:15:15; 85:5:10; and 80:5:15.

[0054] The desirable properties of the multilayer film facestocks of thepresent invention are improved, particularly with regard to machinedirection Gurley stiffness and die-cuttability, when at least the baselayer, and more preferably, the entire multilayered film of thefacestock, has been oriented in the machine direction only. Generally,the base layer and/or entire multilayer film will be oriented in themachine direction at a stretch ratio of at least about 2:1, and morepreferably at a stretch ratio of from about 3:1 to about 9:1. In anotherpreferred embodiment, the film is oriented in a machine direction at aratio of about 4:1 to about 6:1. The oriented film is then preferablyheat set or annealed to provide dimensional stability (i.e., to preventshrinking, relaxing or any distortion of the film).

[0055] In one embodiment, the composition of the second skin layer willbe different from the composition of the first skin layer, and, in thisembodiment, the second skin layer may comprise a polyethylene that isdifferent from the polyethylene used in the first skin layer (includinglow and medium density polyethylenes) or a thermoplastic film formingpolymer that is not a polyethylene having a density of about 0.940 g/cm³or less. Examples of thermoplastic film forming polymers that can beutilized in the second skin layer, either alone or in combinationinclude polyolefins (linear or branched), polyamides, polystyrenes,nylon, polyesters, polyester copolymers, polyurethanes, polysulfones,polyvinylidine chloride, styrene-maleic anhydride copolymers,styrene-acrylonitrile copolymers, ionomers based on sodium or zinc saltsof ethylene methacrylic acid, polymethyl methacrylates, cellulosics,fluoroplastics, acrylic polymers and copolymers, polycarbonates,polyacrylonitriles, and ethylene-vinyl acetate copolymers. Specificexamples of thermoplastics useful as the second skin layer includeacrylates such as ethylene methacrylic acid, ethylene methyl acrylate,ethylene acrylic acid and ethylene ethyl acrylate.

[0056] In one embodiment, the second skin layer comprises a mixture of apolyethylene and a propylene homopolymer or copolymer. The selection ofa particular polymer for the second skin layer is dependent on theproperties and characteristics that are to be added by the presence ofthe second skin layer. The polymer for the second skin layer should becompatible with the polymer of the base layer to provide sufficientadhesion to the base layer in the absence of a tie layer. For example,if the base layer contains a propylene polymer, a second skin layercomprising at least some propylene polymer will adhere to the base layerwithout an intermediate tie layer. It also has been discovered that theuse of a composition in the second skin layer that is different from thecomposition of the first skin layer reduces the blocking tendency whenthe facestock is rolled on itself.

[0057] In one embodiment, the second skin layer comprise a polymer thatis softer than the propylene polymer or copolymer, or blends ofpropylene polymers and copolymers used in the base layer, particularlywhen the second skin layer is joined with an adhesive to a releasecoated liner. In particular, it is preferred that the material of thesecond skin layer has a lower tensile modulus than the tensile modulusof the material comprising the base layer. The use of a lower tensilemodulus second skin layer results in a facestock exhibiting improveddie-cuttability when compared to a facestock wherein the material of thesecond skin layer has a higher tensile modulus than the material of thebase layer.

[0058] In one embodiment, the conformable facestock comprises apolymeric film having an upper surface and a lower surface, aholographic layer on the upper surface of the polymeric film and aprotective layer on the upper surface of the holographic layer. Thepolymeric film may be a monolayer or a multilayer film. The protectivelayer may be a film of the same polymeric compositions described hereinin relation to the polymeric film. The protective film may be laminatedto the holographic layer with adhesive or may be heat sealed onto theholographic layer. Alternatively, the protective layer may comprise acured resin coating applied to the holographic layer. The protectivelayer may provide anti-static properties, abrasion-resistance,UV-blocking properties, etc. to the facestock. The protective layer istransparent and conformable.

[0059] Labelstock

[0060] The above-described facestocks containing the hologram are usefulas labels. As illustrated in FIG. 4, label 40 is made up of polymericfilm 41 having an upper surface and a lower surface, and holographiclayer 42 having image 43 adhered to the lower surface of polymeric film41. Optional reflective material 44 is coated over the lower surface ofthe holographic layer 42. Holographic layer 42 (optionally with thereflective material) is adhered to adhesive 45, which in turn isreleasably adhered to release liner 46.

[0061]FIG. 5 illustrates yet another embodiment of the present inventionthat relates to a multilayer labelstock for use in preparing adhesivelabels. The labelstock 50 comprises a multilayer film polymeric film 51having skin layers 53 and 54 adhered to the surfaces of base layer 52.The second skin layer 54 is also adhered to holographic layer 55 havingimage 56. Holographic layer 55 is adhered to adhesive 57, which in turnis releasably adhered to release liner 58. The multilayer film facestock51 of FIG. 5 is similar to the multilayer facestock of FIG. 3. Thepresent invention also contemplates adhesive multilayer labelstocks thatcomprise multilayer film facestocks having one, two, three or even fourlayers and an adhesive layer. Such labelstocks can be illustrated byadding an adhesive layer to the facestocks illustrated in FIGS. 1-3where the adhesive layer is in contact with the exposed surface of theholographic layers 12, 22, and 32 in FIGS. 1, 2 and 3, respectively.

[0062] In another embodiment illustrated in FIG. 6, the labelstock 60comprises a polymeric film 61 having an upper surface and a lowersurface, holographic layer 62 with image 63 adhered to the upper surfaceof polymeric film 61, and protective layer 64 adhered to the uppersurface of holographic layer 62. An adhesive layer 65 is adhered to thelower surface of polymeric film 61 and releasably adhered to releaseliner 66. Polymeric film 61 may be a monolayer or a multilayer film.

[0063] The labelstock of the present invention generally has an overallthickness of up to about 20 mils. In one embodiment, the thickness ofthe labelstock is from about 0.6 mils to about 12 mils.

[0064] Typically, the adhesive layer has a thickness in the range offrom about 0.1 to about 2 mils (2.5 to 50 microns). Adhesives suitablefor use in labelstocks of the present invention are commonly availablein the art. Generally, these adhesives include pressure-sensitiveadhesives, heat-activated adhesives, hot melt adhesives, and the like.Pressure-sensitive adhesives are particularly preferred. These includeacrylic based adhesives as well as other elastomers such as naturalrubber or synthetic rubbers containing polymers or copolymers ofstyrene, butadiene, acrylonitrile, isoprene and isobutylene.Pressure-sensitive adhesives are well known in the art and any of theknown adhesives can be used with the facestocks of the presentinvention. In one preferred embodiment, the pressure-sensitive adhesivesare based on copolymers of acrylic acid esters, such as, for example,2-ethyl hexyl acrylate, with polar comonomers such as acrylic acid.

[0065] Adhesives that are tacky at any temperature up to about 160° C.(about 320° F.) are particularly useful. PSAs that are tacky at ambienttemperatures are particularly useful in the coextruded adhesiveconstructions of the present invention. A variety of conventional PSAscan be utilized provided that the viscosity is or can be modified to besimilar to the viscosity of the polymeric film material that is beingcoextruded with the adhesive. Useful PSA compositions are fluid orpumpable at the temperatures used in the melt processing. Also, theadhesive compositions should not significantly degrade or gel at thetemperature employed and over the time required for melt processing andextrusion. Typically, the adhesive compositions have a viscosity of from1000 poise to 1,000,000 poise at the processing temperature.

[0066] The adhesives may generally be classified into the followingcategories:

[0067] Random copolymer adhesives such as those based upon acrylateand/or methacrylate copolymers, a-olefin copolymers, siliconecopolymers, chloroprene/acrylonitrile copolymers, and the like,

[0068] Block copolymer adhesives including those based upon linear blockcopolymers (i.e., A-B and A-B-A type), branched block copolymers, starblock copolymers, grafted or radial block copolymers, and the like, andNatural and synthetic rubber adhesives.

[0069] A description of useful pressure-sensitive adhesives may be foundin Encyclopedia of Polymer Science and Engineering, Vol.13.Wiley-Interscience Publishers (New York, 1988). Additional descriptionof useful pressure-sensitive adhesives may be found in Encyclopedia ofPolymer Science and Technology, Vol. 1, Interscience Publishers (NewYork, 1964).

[0070] Commercially available pressure-sensitive adhesives are useful inthe invention. Examples of these adhesives include the hot meltpressure-sensitive adhesives available from H. B. Fuller Company, St.Paul, Minn. as HM-1 597, HL-2207-X, HL-2115X, HL-2193-X. Other usefulcommercially available pressure-sensitive adhesives include thoseavailable from Century Adhesives Corporation, Columbus, Ohio.

[0071] Conventional PSAs, including silicone-based PSAs, rubber-basedPSAs, and acrylic-based PSAs are useful. Another commercial example of ahot melt adhesive is H2187-01, sold by Ato Findley, Inc., of Wauwatusa,Wis. In addition, rubber based block copolymer PSAs described in U.S.Pat. No. 3,239,478 (Harlan) also can be utilized in the coextrudedadhesive constructions of the present invention, and this patent ishereby incorporated by a reference for its disclosure of such hot meltadhesives.

[0072] In one preferred embodiment, the pressure sensitive adhesiveutilized in the present invention comprise rubber based elastomermaterials such as linear, branched, grafted, or radial block copolymersrepresented by the diblock structures A-B, the triblock A-B-A, theradial or coupled structures (A-B)_(n), and combinations of these whereA represents a hard thermoplastic phase or block that is non-rubbery orglassy or crystalline at room temperature but fluid at highertemperatures, and B represents a soft block that is rubbery orelastomeric at service or room temperature. These thermoplasticelastomers may comprise from about 75% to about 95% by weight of rubberysegments and from about 5% to about 25% by weight of non-rubberysegments.

[0073] The non-rubbery segments or hard blocks comprise polymers ofmono- and polycyclic aromatic hydrocarbons, and more particularlyvinyl-substituted aromatic hydrocarbons that may be monocyclic orbicyclic in nature. The preferred rubbery blocks or segments are polymerblocks of homopolymers or copolymers of aliphatic conjugated dienes.Rubbery materials such as polyisoprene, polybutadiene, and styrenebutadiene rubbers may be used to form the rubbery block or segment.Particularly preferred rubbery segments include polydienes and saturatedolefin rubbers of ethylene/butylene or ethylene/propylene copolymers.The latter rubbers may be obtained from the corresponding unsaturatedpolyalkylene moieties such as polybutadiene and polyisoprene byhydrogenation thereof.

[0074] The block copolymers of vinyl aromatic hydrocarbons andconjugated dienes that may be utilized include any of those that exhibitelastomeric properties. The block copolymers may be diblock, triblock,multiblock, starblock, polyblock or graftblock copolymers. Throughoutthis specification and claims, the terms diblock, triblock, multiblock,polyblock, and graft or grafted-block with respect to the structuralfeatures of block copolymers are to be given their normal meaning asdefined in the literature such as in the Encyclopedia of Polymer Scienceand Engineering, Vol. 2, (1985) John Wiley & Sons, Inc., New York, pp.325-326, and by J. E. McGrath in Block Copolymers, Science Technology,Dale J. Meier, Ed., Harwood Academic Publishers, 1979, at pages 1-5.

[0075] Such block copolymers may contain various ratios of conjugateddienes to vinyl aromatic hydrocarbons including those containing up toabout 40% by weight of vinyl aromatic hydrocarbon. Accordingly,multi-block copolymers may be utilized that are linear or radialsymmetric or asymmetric and that have structures represented by theformulae A-B, A-B-A, A-B-A-B, B-A-B, (AB)_(0,1,2) . . . BA, etc.,wherein A is a polymer block of a vinyl aromatic hydrocarbon or aconjugated diene/vinyl aromatic hydrocarbon tapered copolymer block, andB is a rubbery polymer block of a conjugated diene.

[0076] The block copolymers may be prepared by any of the well-knownblock polymerization or copolymerization procedures including sequentialaddition of monomer, incremental addition of monomer, or couplingtechniques as illustrated in, for example, U.S. Pat. Nos. 3,251,905;3,390,207; 3,598,887; and 4,219,627. As well known, tapered copolymerblocks can be incorporated in the multi-block copolymers bycopolymerizing a mixture of conjugated diene and vinyl aromatichydrocarbon monomers utilizing the difference in their copolymerizationreactivity rates. Various patents describe the preparation ofmulti-block copolymers containing tapered copolymer blocks includingU.S. Pat. Nos. 3,251,905; 3,639,521; and 4,208,356, the disclosures ofwhich are hereby incorporated by reference.

[0077] Conjugated dienes that may be utilized to prepare the polymersand copolymers are those containing from 4 to about 10 carbon atoms andmore generally, from 4 to 6 carbon atoms. Examples include from1,3-butadiene, 2-methyl-1,3-butadiene (isoprene),2,3-dimethyl-1,3-butadiene, chloroprene, 1,3-pentadiene, 1,3-hexadiene,etc. Mixtures of these conjugated dienes also may be used. The preferredconjugated dienes are isoprene and 1,3-butadiene.

[0078] Examples of vinyl aromatic hydrocarbons that may be utilized toprepare the copolymers include styrene and the various substitutedstyrenes such as o-methylstyrene, p-methylstyrene, p-tert-butylstyrene,1,3-dimethylstyrene, alpha-methylstyrene, beta-methylstyrene,p-isopropylstyrene, 2,3-dimethylstyrene, o-chlorostyrene,p-chlorostyrene, o-bromostyrene, 2-chloro-4-methylstyrene, etc. Thepreferred vinyl aromatic hydrocarbon is styrene.

[0079] Many of the above-described copolymers of conjugated dienes andvinyl aromatic compounds are commercially available. The number averagemolecular weight of the block copolymers, prior to hydrogenation, isfrom about 20,000 to about 500,000, preferably from about 40,000 toabout 300,000.

[0080] The average molecular weights of the individual blocks within thecopolymers may vary within certain limits. In most instances, the vinylaromatic block will have a number average molecular weight in the orderof about 2000 to about 125,000, and preferably between about 4000 and60,000. The conjugated diene blocks either before or after hydrogenationwill have number average molecular weights in the order of about 10,000to about 450,000 and more preferably from about 35,000 to 150,000.

[0081] Also, prior to hydrogenation, the vinyl content of the conjugateddiene portion generally is from about 10% to about 80%, and the vinylcontent is preferably from about 25% to about 65%, particularly 35% to55% when it is desired that the modified block copolymer exhibit rubberyelasticity. The vinyl content of the block copolymer can be measured bymeans of nuclear magnetic resonance.

[0082] Specific examples of diblock copolymers include styrene-butadiene(SB), styrene-isoprene (SI), and the hydrogenated derivatives thereof.Examples of triblock polymers include styrene-butadiene-styrene (SBS),styrene-isoprene-styrene (SIS),alpha-methylstyrene-butadiene-alpha-methylstyrene, andalpha-methylstyrene-isoprene alpha-methylstyrene. Examples ofcommercially available block copolymers useful as the adhesives in thepresent invention include those available from Shell Chemical Companyand listed in the following Table III. TABLE III Styrene/Rubber MeltKraton Type Ratio (w) Index D1101 Linear SBS 31/69 <1 D1107P Linear SIS15/85 11 D1111 Linear SIS 22/78 3 D1112P Linear SIS 15/85 23 D1113PLinear SIS 16/84 24 D1117P Linear SIS 17/83 33 D1320X Multi-arm (SI)_(n)10/90 NA

[0083] Vector 4111 is a SIS block copolymer available from Dexco ofHouston, Tex.

[0084] Upon hydrogenation of the SBS copolymers comprising a rubberysegment of a mixture of 1,4 and 1,2 isomers, a styrene-ethylene-butylenestyrene (SEBS) block copolymer is obtained. Similarly, hydrogenation ofan SIS polymer yields a styrene-ethylene propylene-styrene (SEPS) blockcopolymer.

[0085] The selective hydrogenation of the block copolymers may becarried out by a variety of well known processes including hydrogenationin the presence of such catalysts as Raney nickel, noble metals such asplatinum, palladium, etc., and soluble transition metal catalysts.Suitable hydrogenation processes that can be used are those wherein thediene-containing polymer or copolymer is dissolved in an inerthydrocarbon diluent such as cyclohexane and hydrogenated by reactionwith hydrogen in the presence of a soluble hydrogenation catalyst. Suchprocedures are described in U.S. Pat. Nos. 3,113,986 and 4,226,952, thedisclosures of which are incorporated herein by reference. Suchhydrogenation of the block copolymers that are carried out in a mannerand to extent as to produce selectively hydrogenated copolymers having aresidual unsaturation content in the polydiene block of from about 0.5%to about 20% of their original unsaturation content prior tohydrogenation.

[0086] In one embodiment, the conjugated diene portion of the blockcopolymer is at least 90% saturated and more often at least 95%saturated while the vinyl aromatic portion is not significantlyhydrogenated. Particularly useful hydrogenated block copolymers arehydrogenated products of the block copolymers ofstyrene-isoprene-styrene such as a styrene-(ethylene/propylene)-styreneblock polymer. When a polystyrene-polybutadiene-polystyrene blockcopolymer is hydrogenated, it is desirable that the 1,2-polybutadiene to1,4-polybutadiene ratio in the polymer is from about 30:70 to about70:30. When such a block copolymer is hydrogenated, the resultingproduct resembles a regular copolymer block of ethylene and 1-butene(EB). As noted above, when the conjugated diene employed as isoprene,the resulting hydrogenated product resembles a regular copolymer blockof ethylene and propylene (EP).

[0087] A number of selectively hydrogenated block copolymers areavailable commercially from Shell Chemical Company under the generaltrade designation “Kraton G.” One example is Kraton G1652 which is ahydrogenated SBS triblock comprising about 30% by weight of styrene endblocks and a midblock that is a copolymer of ethylene and 1-butene (EB).A lower molecular weight version of G1652 is available from Shell underthe designation Kraton G1650. Kraton G1651 is another SEBS blockcopolymer that contains about 33% by weight of styrene. Kraton G1657 isan SEBS diblock copolymer that contains about 13%w styrene. This styrenecontent is lower than the styrene content in Kraton G1650 and KratonG1652.

[0088] In another embodiment, the selectively hydrogenated blockcopolymer is of the formula

B _(n)(AB)_(o) A _(p)

[0089] wherein

[0090] n=0 or 1;

[0091] o is 1 to 100;

[0092] p is 0 or 1;

[0093] each B prior to hydrogenation is predominantly a polymerizedconjugated diene hydrocarbon block having a number average molecularweight of about 20,000 to about 450,000;

[0094] each A is predominantly a polymerized vinyl aromatic hydrocarbonblock having a number average molecular weight of from about 2000 toabout 115,000; the blocks of A constituting about 5% to about 95% byweight of the copolymer; and the unsaturation of the block B is lessthan about 10% of the original unsaturation.

[0095] In other embodiments, the unsaturation of block B is reduced uponhydrogenation to less than 5% of its original value, and the averageunsaturation of the hydrogenated block copolymer is reduced to less than20% of its original value.

[0096] The block copolymers may also include functionalized polymerssuch as may be obtained by reacting an alpha, beta-olefinicallyunsaturated monocarboxylic or dicarboxylic acid reagent onto selectivelyhydrogenated block copolymers of vinyl aromatic hydrocarbons andconjugated dienes as described above. The reaction between thecarboxylic acid reagent in the graft block copolymer can be effected insolutions or by a melt process in the presence of a free radicalinitiator.

[0097] The preparation of various selectively hydrogenated blockcopolymers of conjugated dienes and vinyl aromatic hydrocarbons thathave been grafted with a carboxylic acid reagent is described in anumber of patents including U.S. Pat. Nos. 4,578,429; 4,657,970; and4,795,782, and the disclosures of these patents relating to graftedselectively hydrogenated block copolymers of conjugated dienes and vinylaromatic compounds, and the preparation of such compounds are herebyincorporated by reference. U.S. Pat. Nos. 4,795,782 describes and givesexamples of the preparation of the grafted block copolymers by thesolution process and the melt process. U.S. Pat. Nos. 4,578,429 containsan example of grafting of Kraton G1652 (SEBS) polymer with maleicanhydride with 2,5-dimethyl-2,5-di(t-butylperoxy) hexane by a meltreaction in a twin screw extruder. (See Col. 8, lines 40-61.)

[0098] Examples of commercially available maleated selectivelyhydrogenated copolymers of styrene and butadiene include Kraton FG1901X,FG1921X, and FG1924X from Shell, often referred to as maleatedselectively hydrogenated SEBS copolymers. FG1901X contains about 1.7% byweight bound functionality as succinic anhydride and about 28% w ofstyrene. FG1921X contains about 1% w of bound functionality as succinicanhydride and 29% w of styrene. FG1924X contains about 13% styrene andabout 1% bound functionality as succinic anhydride.

[0099] Useful block copolymers also are available from Nippon Zeon Co.,2-1, Marunochi, Chiyoda-ku, Tokyo, Japan. For example, Quintac 3530 isavailable from Nippon Zeon and is believed to be a linearstyrene-isoprene-styrene block copolymer.

[0100] The polymer film materials and adhesive compositions used to formthe constructions of the present invention may be neat, or they may beemulsions or solvent-based. Emulsion and solvent-based acrylic basedPSAs are known and described in, for example, U.S. Pat. Nos. 5,639,811and 5,164,444, respectively, and these patents are hereby incorporatedby reference for such disclosures.

[0101] The present labelstock has sufficient stiffness for gooddispensing and matrix stripping. Orientation of the multilayer filmfacestocks in the machine direction increases the tensile modulus in themachine direction which contributes to dimensional stability and goodprint registration. The multilayer film facestocks of the presentinvention can be oriented in the machine direction by procedures wellknown to those skilled in the art such as by hot stretching themultilayer film facestock at a stretch ratio of at least 2, andgenerally at a stretch ratio from about 2 to about 9. After passingaround preheated rolls that soften the facestock, the softened facestockis then stretched and thereafter annealed or heat-set, and finally,cooled over a chill roll to complete the hot stretch operation. Thefacestock may then be taken up in roll form and stored.

[0102] In the manufacture of labelstock from the above-describedmultilayer film facestocks in accordance with the invention, liner orcarrier stock may be provided. The liner or carrier stock may comprise amultilayer liner made for example as disclosed in U.S. Pat. No.4,713,273, the entire disclosure of which is incorporated herein byreference, or may be a conventional liner or carrier consisting of asingle paper of film layer that may be supplied in roll form. If it hasnot been previously provided with a release coating and does not itselfinclude components to inherently generate a release surface at itsadhesive-contacting face, the liner or carrier may be coated with arelease coating (e.g., a silicone). If a release coating is applied, itis dried or cured following application by any suitable means.

[0103] The release face of the release liner or carrier may be coatedwith a layer of pressure-sensitive adhesive for subsequent transfer ofthe adhesive to the facestock with which the liner or carrier isemployed. When the facestock is combined with the liner or carrier, theadhesive is joined to the facestock. Later, the liner or carrier isremoved to expose the adhesive, and the adhesive remains permanentlyjoined to the facestock.

[0104] In some applications, the adhesive layer may be a heat-activatedadhesive or a hot-melt adhesive such as used in in-mold labelapplications, as distinguished from a pressure-sensitive adhesive. Ifthe adhesive is a heat-activated adhesive or a hot-melt adhesive, theremay be no need for the provision of a release liner for inherentreleasability such as is required when using a pressure-sensitiveadhesive.

[0105] While the invention has been explained in relation to itspreferred embodiments, it is to be understood that various modificationsthereof will become apparent to those skilled in the art upon readingthe specification. Therefore, it is to be understood that the inventiondisclosed herein is intended to cover such modifications as fall withinthe scope of the appended claims.

1. A conformable facestock comprising a polymeric film having an uppersurface and a lower surface, and a holographic layer having an uppersurface and a lower surface, wherein the upper surface of theholographic layer is adhered to the lower surface of the polymeric film.2. The conformable facestock of claim 1 wherein the holographic layercomprises a cured casting resin and a reflective material overlying atleast a portion of the casting resin.
 3. The conformable facestock ofclaim 2 wherein the casting resin has at least one image therein.
 4. Theconformable facestock of claim 2 wherein the reflective material coversthe entire surface of the casting resin.
 5. The conformable facestock ofclaim 3 wherein the reflective material covers the portion of thecasting resin having the image therein.
 6. The conformable facestock ofclaim 1 wherein the polymeric film is selected from the group consistingof a polystyrene, a polyolefin, a polyamide, a polyester, apolycarbonate, a polyvinyl alcohol, a poly(ethylene vinyl alcohol), apolyurethane, a polyacrylate, a poly(vinyl acetate), an ionomer andmixtures thereof.
 7. The conformable facestock of claim 1 wherein thepolymeric film comprises a polyolefin.
 8. The conformable facestock ofclaim 1 wherein the polymeric film comprises a monolayer film.
 9. Theconformable facestock of claim 1 wherein the polymeric film comprises amultilayer film.
 10. The conformable facestock of claim 9 wherein themultilayer film comprises a base layer having an upper surface and alower surface, and at least a first skin layer bonded to the uppersurface of the base layer.
 11. The conformable facestock of claim 10wherein the base layer comprises (a) a polyethylene, (b) a propylenehomopolymer or copolymer, or (c) a blend of (i) a polyethylene or apropylene homopolymer and (i) at least one propylene copolymer.
 12. Theconformable facestock of claim 11 wherein the base layer comprises apropylene homopolymer.
 13. The conformable facestock of claim 11 whereinthe propylene copolymer of the base layer comprises a copolymer ofpropylene and up to about 40% by weight of at least one α-olefinselected from ethylene and α-olefins containing from 4 to about 8 carbonatoms.
 14. The conformable facestock of claim 13 wherein the a-olefincomprises ethylene, 1-butene, or 1-octene.
 15. The conformable facestockof claim 11 wherein the base layer comprises a blend of (a) a propylenehomopolymer and (b) a propylene-ethylene or a propylene-1-butenecopolymer.
 16. The conformable facestock of claim 10 wherein the skinlayer comprises a blend of (a) a polyethylene, (b) a propylenehomopolymer and (c) a propylene-ethylene or a propylene-1-butenecopolymer.
 17. The conformable facestock of claim 11 wherein the baselayer further comprises at least one nucleating agent.
 18. Theconformable facestock of claim 10 wherein the base layer is oriented inthe machine direction at a stretch ratio of from about 3:1 to about 9:1.19. The conformable facestock of claim 10 wherein the base layer isoriented in the machine direction at a stretch ratio of at least about2:1.
 20. The conformable facestock of claim 1 wherein the polymeric filmis oriented in the machine direction at a stretch ratio of from about3:1 to about 9:1.
 21. The conformable facestock of claim 9 wherein thepolymeric film comprises a coextruded film.
 22. The conformablefacestock of claim 10 further comprising a second skin layer bonded tothe lower surface of the base layer.
 23. The conformable facestock ofclaim 22 wherein the composition of the second skin layer is differentfrom the composition of the first skin layer.
 24. The conformablefacestock of claim 22 wherein the composition of the second skin layeris essentially the same as the composition of first skin layer.
 25. Theconformable facestock of claim 22 wherein the second skin layercomprises a thermoplastic polymer.
 26. The conformable facestock ofclaim 22 wherein the second skin layer comprises at least one polymerselected from the group of polyolefins, polyamides, polystyrenes,polystyrene-butadiene, polyesters, polyester copolymers, polyurethanes,polysulfones, polyvinylidene chloride, styrene-maleic anhydridecopolymers, styrene acrylonitrile copolymers, ionomers based on sodiumor zinc salts of ethylene methacrylic acid, polymethylmethacrylates,cellulosics, fluoroplastics, acrylic polymers and copolymers,polycarbonates, polyacrylonitriles, ethylene-vinyl acetate copolymers,and mixtures thereof.
 27. The conformable facestock of claim 22 whereinthe second skin layer comprises a mixture of a polyethylene and apropylene homopolymer or copolymer.
 28. The conformable facestock ofclaim 22 wherein the second skin layer is bonded to the lower surface ofthe base layer through a tie layer.
 29. The conformable facestock ofclaim 28 wherein the composition of the second skin layer is differentfrom the composition of the first skin layer.
 30. The conformablefacestock of claim 28 wherein the second skin layer comprises at leastone polymer selected from the group of polyolefins, polyamides,polystyrenes, polystyrene-butadienes, polyesters, polyester copolymers,polyurethanes, polysulfones, polyvinylidene chloride, styrene-maleicanhydride copolymers, styrene acrylonitrile copolymers, ionomers basedon sodium or zinc salts of ethylene methacrylic acid,polymethylmethacrylates, cellulosics, fluoroplastics, acrylic polymersand copolymers, polycarbonates, polyacrylonitriles, ethylene-vinylacetate copolymers, and mixtures thereof.
 31. The conformable facestockof claim 28 wherein the polymeric film is oriented in the machinedirection at a stretch ratio of at least about 2:1.
 32. The conformablefacestock of claim 28 wherein the polymeric film comprises a coextrudedfilm.
 33. The conformable facestock of claim 32 wherein the polymericfilm is oriented in the machine direction at a stretch ratio of fromabout 3:1 to about 9:1.
 34. The conformable facestock of claim 8 whereinthe polymeric film comprises a blend of (a) a propylene homopolymer orcopolymer and (b) an alkylene-alkyl-acrylate or methacrylate copolymer;wherein the polymeric film is machine direction oriented.
 35. Theconformable facestock of claim 34 wherein the alkylene of (b) is anα-olefin containing from 2 to 8 carbon atoms.
 36. The conformablefacestock of claim 34 wherein the alkyl-acrylate of (b) is a C₁ to C₈alkyl acrylate or methacrylate.
 37. The conformable facestock of claim34 wherein (b) is ethylene butylacrylate copolymer.
 38. The conformablefacestock of claim 1 wherein the thickness of the polymeric film is fromabout 0.5 mils to about 10 mils.
 39. The conformable facestock of claim1 wherein the thickness of the polymeric film is less than about 6 mils.40. The conformable facestock of claim 1 further comprising a protectivelayer overlying the lower surface of the holographic layer.
 41. Aconformable labelstock for use in adhesive labels comprising: aconformable facestock comprising a polymeric film having an uppersurface and a lower surface and a holographic layer having an uppersurface and a lower surface, wherein the upper surface of theholographic layer is adhered to the lower surface of the polymeric film;and an adhesive layer having an upper surface and a lower surface,wherein the upper surface of the adhesive layer is adhered to the lowersurface of the holographic layer.
 42. A conformable labelstock for usein adhesive labels comprising: a conformable facestock comprising apolymeric film having an upper surface and a lower surface and aholographic layer having an upper surface and a lower surface, whereinthe upper surface of the holographic layer is adhered to the lowersurface of the polymeric film; and an adhesive layer having an uppersurface and lower surface, wherein the lower surface of the adhesivelayer is adhered to the upper surface of the polymeric film.
 43. Theconformable labelstock of claim 42 further comprising a protective layeradhered to the lower surface of the holographic layer.
 44. Theconformable labelstock of claim 41 wherein the adhesive is a pressuresensitive adhesive.
 45. The conformable labelstock of claim 42 whereinthe adhesive is a pressure sensitive adhesive.
 46. The conformablelabelstock of claim 41 further comprising a release liner releasablyadhered to the lower surface of the adhesive layer.
 47. The conformablelabelstock of claim 42 further comprising a release liner releasablyadhered to the upper surface of the adhesive layer.
 48. A conformablelabelstock for use in adhesive labels comprising: (a) a multilayerconformable facestock comprising a base layer having an upper surfaceand a lower surface, a first skin layer bonded to the upper surface ofthe base layer by a tie layer, and a holographic layer on the lowersurface of the base layer; wherein the base layer comprises (i) apropylene homopolymer or copolymer, or (ii) a blend of a propylenehomopolymer and at least one propylene copolymer; (b) an adhesive layerhaving an upper surface and a lower surface wherein the upper surface ofthe adhesive layer is adhesively joined to the holographic layer. 49.The conformable labelstock of claim 48 having a thickness up to about 20mils.
 50. The conformable labelstock of claim 48 having a thickness offrom about 0.6 to about 12 mils.
 51. The conformable labelstock of claim48 further comprising a release coated liner in contact with andreleasably joined to the lower surface of the adhesive layer.
 52. Alabel made from the conformable facestock of claim
 1. 53. A pressuresensitive adhesive label die-cut from the conformable labelstock ofclaim
 41. 54. A pressure sensitive adhesive label die-cut from theconformable labelstock of claim 42.